Single Transition Metal Atom Anchored in C3b a Efficient and Selective Electrocatalyst for Nitrogen Reduction Reaction

Electrocatalytic nitrogen reduction reaction (NRR), the conversion of N2 to ammonia under mild conditions, represents a highly promising new technology. Adoption of the density function theory (DFT) calculations, we systematically explored the feasibility of TM@C3B (TM = Sc-Zn, Y-Cd, Lu-Hg) as a catalyst for ammonia synthesis. Electronic structure analysis indicates that hybridization between N-p and TM-d orbitals forms lower energy antibond orbitals to enhance N2 adsorption, while activation the N−N triple bond. The single Mo atom anchored in C3B possess the optimal catalytic performance among all TM atoms anchored, with a limiting potential of 0.32V for *N2-*NNH in the Distal channel. In addition, the competitive two-electron hydrogen evolution reaction (HER) was adequately alleviated in the progress of NRR. This work may open up potential avenues for artificial ammonia synthesis with single-atom catalysts under mild conditions.